Abstract

In batteries, like all electrochemical systems, interfacial phenomena play a critical role in thermodynamic stability, charge transfer kinetics, and ionic transport phenomena. For example, in Li-ion batteries, the solid-electrolyte interphase (SEI) layer enables stabilization of liquid electrolytes against continual electrolyte decomposition. In solid-state batteries, the dynamic morphological evolution of the interface results in unique electro-chemo-mechanical properties, which dictate performance, degradation, and ultimate failure.As a result of these coupled phenomena, there is a continued need to improve both our fundamental understanding of interfacial dynamics, as well as new strategies to engineer rationally-controlled interfaces. Among the various interfacial engineering methodologies, atomic layer deposition (ALD) has risen in interest in recent years, owing to its unparalleled ability to impart atomically-precise control of surface composition and structure, while maintaining conformal coating of ultra-high aspect ratio structures.In this talk, I will describe recent progress in applying ALD for battery applications. In the field of Li-ion batteries, I will show how deposition of a single-ion conducting solid electrolyte on the surface of graphite anodes can eliminate electrolyte decomposition and SEI formation, resulting in a four-fold decrease in interfacial resistance [1]. This results in lower cell polarization during fast charging, eliminating deleterious Li plating on the anode. In the field of Li metal batteries, I will also show how ALD coatings can influence nucleation and growth, resulting in improved Coulombic efficiency [2]. Finally, I will describe efforts towards incorporation of ALD films into solid-state batteries, where mechanical properties play a critical role [3-4].[1] E. Kazyak, K.-H. Chen, Y. Chen, T. H. Cho, N. P. Dasgupta, Adv. Energy Mater. 12, 2102618 (2022).[2] K.-H. Chen, A. J. Sanchez, E. Kazyak, A. L. Davis, N. P. Dasgupta, Adv. Energy Mater. 9, 1802534 (2019).[3] A. L. Davis, R. Garcia-Mendez, K. N. Wood, E. Kazyak, K.-H. Chen, G. Teeter, J. Sakamoto, N. P. Dasgupta, J. Mater. Chem. A 8, 6291 (2020)[4] E. Kazyak, M. Shin, W. S. LePage, T. H. Cho, N. P. Dasgupta, Chem. Commun. 56, 15537 (2020).

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